Bimetallic NiMnOx catalysts enable cascade C–H and C–C bond cleavage for efficient low-temperature ethane oxidation

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Qianqian Gao , Jiali Tang , Jinhang Yang , Beilong Lin , Peirong Chen , Mingli Fu , Daiqi Ye , Yun Hu
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Abstract

Transition metal oxide catalysts offer a cost-effective and efficient alternative to noble metal catalysts for the environmental treatment of light alkane pollutants. In this study, a bimetallic Ni0.2Mn0.8Ox catalyst was evaluated for its effectiveness in the low-temperature catalytic oxidation of ethane, which achieved an ethane conversion of 90 % at only 286 °C and exceeded 99 % at 325 °C. Under conditions of poisoning with 5 vol% H2O or 10 ppm H2S for 10 h, the activity of the Ni0.2Mn0.8Ox catalyst remained essentially unchanged. The characterization results indicated that the Ni sites on the surface of Ni0.2Mn0.8Ox were favorable for the adsorption of ethane. Simultaneously introducing Ni promoted lattice distortion in MnOx and increased the exposure of lattice oxygen to participate in the reaction. In mechanistic studies, it was elucidated that the Ni sites play a distinct role in facilitating the scission of C–H bonds, while the Mn sites exhibit a specific propensity towards breaking C–C bonds. The synergistic effect between Ni and Mn sites promoted the activation of ethane on the surface of Ni0.2Mn0.8Ox and decomposing into H2O and CO2 under the function of lattice oxygen. The monolithic catalysts demonstrated long-term stability, maintaining removal rates of ethane above 85 % under dry conditions and 75 % under wet conditions for up to 100 h. This performance suggests significant potential for industrial applications.

Abstract Image

Abstract Image

双金属NiMnOx催化剂能够级联C-H和C-C键裂解,实现高效的低温乙烷氧化
过渡金属氧化物催化剂为轻烷烃污染物的环境处理提供了一种经济高效的贵金属催化剂替代品。在本研究中,对双金属Ni0.2Mn0.8Ox催化剂在乙烷低温催化氧化中的有效性进行了评价,该催化剂在286 °C时的乙烷转化率为90 %,在325 °C时的乙烷转化率超过99 %。在5 vol% H2O或10 ppm H2S中毒10 h的条件下,Ni0.2Mn0.8Ox催化剂的活性基本保持不变。表征结果表明,Ni0.2Mn0.8Ox表面的Ni位点有利于乙烷的吸附。同时引入Ni促进了MnOx中的晶格畸变,增加了晶格氧参与反应的暴露量。机理研究表明,Ni位点在促进C-H键断裂中起着明显的作用,而Mn位点则表现出破坏C-C键的特殊倾向。Ni和Mn位点之间的协同作用促进了Ni0.2Mn0.8Ox表面乙烷的活化,并在晶格氧的作用下分解为H2O和CO2。整体催化剂表现出长期的稳定性,在干燥条件下保持乙烷的去除率在85 %以上,在湿条件下保持75 %以上,长达100 h。这一性能表明了工业应用的巨大潜力。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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